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Record W3163620568 · doi:10.1002/jms.4770

Fragmentation reactions of protonated α,ω‐diamino carboxylic acids: The importance of functional group interactions

2021· article· en· W3163620568 on OpenAlexafffund
J. Stuart Grossert, Robert L. White

Bibliographic record

VenueJournal of Mass Spectrometry · 2021
Typearticle
Languageen
FieldChemistry
TopicMass Spectrometry Techniques and Applications
Canadian institutionsDalhousie University
FundersNatural Sciences and Engineering Research Council of Canada
KeywordsChemistryProtonationFragmentation (computing)Medicinal chemistryCarboxylic acidCarbon monoxideSide chainPhotochemistryOrganic chemistryIon

Abstract

fetched live from OpenAlex

Abstract Protonated members of a homologous series of biologically significant α,ω‐diamino carboxylic acids were subjected to collision induced dissociation (CID). The resulting fragmentation patterns were studied using isotopic labeling, quantum mechanical computations, and pseudo MS 3 experiments conducted primarily on an ion trap mass spectrometer. Each protonated α,ω‐diamino acid showed a primary neutral loss of either ammonia or water; a clear explanation was developed for the observed variation of the two losses within the series. Protonated 2,3‐diaminopropanoic acid, 2,4‐diaminobutanoic acid, and 2,7‐diaminoheptanoic acid gave secondary losses of water, carbon monoxide, and a loss of water plus carbon monoxide, respectively. In the parallel pathways characterized for the fragmentations of protonated ornithine and lysine, the α‐nitrogen of the diamino acid was maintained in the cyclic iminium product formed by successive losses of NH 3 and (H 2 O + CO), whereas the side‐chain nitrogen was retained by consecutive losses of H 2 O and (CO, NH 3 ). The 1‐piperideine ion from protonated lysine was fragmented further, losing ethylene from carbons 4 and 5. Protonated 2,6‐diaminopimelic acid fragmented by analogous reactions. Detailed mechanistic schemes for the fragmentation of both protonated 2,3‐diaminopropanoic and ornithine were generated from MP2/DFT computations. This work highlights the participation of the side‐chain amino group, which distinguishes the gas‐phase chemistry of protonated α,ω‐diamino acids from the well‐documented fragmentation reactions of protonated α‐amino acids bearing a hydrogen atom or an alkyl side chain. In general, the results further illustrate the importance of intramolecular separations affecting the specific interactions between functional groups leading to the fragmentation of multifunctional ions.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesInsufficient payload (model declined to judge)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.043
Threshold uncertainty score0.991

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0100.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.016
GPT teacher head0.273
Teacher spread0.257 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations2
Published2021
Admission routes2
Has abstractyes

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